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S CI EN CE OF T H E T OTAL EN V I RO N M EN T 4 0 7 ( 2 0 09 ) 44 3 0–4 43 7

a v a i l a b l e a t w w w. s c i e n c e d i r e c t . c o m

w w w. e l s e v i e r. c o m / l o c a t e / s c i t o t e n v

PCB and organochlorine pesticides in home-produced eggs


in Belgium

I. Windala,⁎, V. Hanota , J. Marchia , G. Huysmansa , I. Van Overmeirea ,


N. Waegeneersb , L. Goeyensa
a
Scientific Institute of Public Health, rue J. Wytsman, B-1050 Brussels, Belgium
b
Veterinary and Agrochemical Research Centre (VAR-CODA-CERVA), Leuvensesteenweg 17, B-3080 Tervuren, Belgium

AR TIC LE D ATA ABSTR ACT

Article history: The level of polychlorinated biphenyls (PCB) and persistent organochlorinated pesticides (OC)
Received 5 August 2008 in home-produced eggs was investigated in Belgium. The concentration of
Received in revised form dichlorodiphenytrichloroethane (DDT) is above the norm for 17% of the eggs collected during
24 November 2008 the spring on 58 different locations. For PCB, aldrin, dieldrin, and chlordane, 3–5% of the
Accepted 25 November 2008 samples are above the norm too. These levels are surprisingly high for compounds banned for
Available online 16 January 2009 about 30 years. Higher concentrations in home-produced eggs are expected compared to
battery eggs because of contact with the environment and especially the soil. For ten selected
Keywords: locations, the concentration in soils, excreta and feed was measured, but no simple correlation
PCB between egg and feed or soil level could be established. Hexachlorohexane, endosulfan, endrin,
Organochlorine pesticides methoxychlor and nitrofen were not detected in any sample.
DDT © 2008 Elsevier B.V. All rights reserved.
Home-produced eggs
Eggs

1. Introduction dichlorodiphenyltrichloroethane (DDT), dieldrin, endrin, hep-


tachlor, mirex, toxaphene, PCB, hexachlorobenzene (HCB),
Persistent Organic Pollutants (POPs) are toxic organic com- dioxins and furans.
pounds resisting biological and chemical degradation. POPs The adverse effects of POPs on the environment and
are characterized by low water solubility and high lipid solu- human health have been well established and led to a
bility, leading to their bioaccumulation in fatty tissues. They reduction of the emission for the first group (e.g., purification
are also semivolatile, enabling them to move long distances in system at the chimney of incinerators) and interdiction of
the atmosphere before deposition occurs (UNEP, 1998). production and use in many countries for most of the
POPs can be classified in two main groups. The first group compounds belonging to the second group (Moniteur belge,
includes POPs which are formed unintentionally in a wide 2006; VITO, 2007). However, the combined properties of POPs
range of manufacturing and combustion processes, like make them still a present issue despite the ban of most
dioxins or polyaromatic hydrocarbons (PAHs). The second compounds since the 1970s. High concentrations of POPs in
group includes POPs which are or have been produced in large the environment, food and feed or human milk and blood are
scale like pesticides or polychlorobiphenyls (PCBs) (some still observed (Smith, 1999; Schecter and Gasiewicz, 2003;
of them have been produced in thousands of tonnes Darnerud et al., 2006; Srogi, 2007; VITO, 2007; Rios et al., 2007;
per year). Twelve chemicals have been defined as Van den Steen et al., 2008). The World Health Organization
POPs in the Stockholm Convention (2001): aldrin, chlordane, (WHO) has proposed Tolerable or Acceptable Daily Intake (TDI

⁎ Corresponding author. Tel.: +32 2 642 51 96; fax: +32 2 642 53 27.
E-mail address: isabelle.windal@iph.fgov.be (I. Windal).

0048-9697/$ – see front matter © 2008 Elsevier B.V. All rights reserved.
doi:10.1016/j.scitotenv.2008.11.063
S CI EN C E OF TH E T OTAL EN V I RO N M EN T 4 0 7 ( 2 0 09 ) 44 3 0–4 43 7 4431

or ADI) or Tolerable Weekly Intake (TWI) for most of these pesticides, trace elements, mycotoxins, polyaromatic
compounds (JMPR, 1994, 2000, 2002; ATSDR, 2002). ADI/TDI/TWI, hydrocarbons, brominated flame retardants such as poly-
properties and year these compounds were banned in Belgium brominated diphenyl ethers (PBDEs), hexabromocyclodo-
are summarized in Table 1 for compounds investigated in this decane (HBCD) and tetrabromobisphenol-A (TBBP-A), PCB
study. metabolites and perfluorinated compounds (PFOA and
Because of their high fat content, eggs are known to PFOS);
accumulate POP and can be considered as a good indicator of 2) investigation of the sources of contamination through
ambient pollution (Jaspers et al., 2006; Schuler et al., 1997). In analyses of soil samples, as well as of kitchen waste
this study, the concentrations of several pesticides (most of given to the hens;
them defined as POPs) and PCBs in eggs from free-range hens 3) realization of an assessment of the risks related to the
of private owners in Belgium have been determined. The consumption of home-produced eggs compared to the
objectives are to assess the level of POPs in a food item which consumption of commercially produced eggs;
is not under the control of the food chain organized at the 4) suggestion of possible measures to reduce contamination
national or European level and evaluate the possible impact of levels and the study of their feasibility.
eggs' consumption on human health. Since it is well known
that, for foraging chickens, soil can be an important source
contamination (Schuler et al., 1997; Van Eijkeren et al., 2006), 2. Materials and methods
soil and feed samples were analyzed at selected locations to
determine the main origin of the contamination. Levels in 2.1. Sampling
excreta were investigated as well. Two sets of measurements
were performed, one in spring and one in autumn, to evaluate Sampling is described in detail in Van Overmeire et al. (2009).
a possible seasonal variation. Briefly, a set of egg samples belonging to private owners was
This study is a part of a general study on egg contamination collected from all over Belgium. Sampling was performed
in Belgium, called CONTEGG. Details on objectives, sampling in the autumn 2006 (40 egg samples) and in the spring 2007
and general conclusions can be found in the paper of Van (58 egg samples; same location than in spring + 18 other
Overmeire et al., accepted for publication in Science of the locations). Private owners were recruited on a voluntary
Total Environment in 2008. The four main aspects of the basis. A set of criteria was used to select the private owners:
CONTEGG project are summarized below: their hens are living in a free-range system, no commercial egg
production occurred, kitchen waste is offered as feed to the
1) determination of the contamination of home-produced eggs hens in addition to commercial feed. The locations where the
in Belgium by dioxins and dioxin-like PCB, marker PCBs, hen holders lived included densely populated surfaces as well
as agricultural areas. Analyses of metals, chlorinated pesti-
cides, marker PCB and dioxin (by Chemically Activated
LUciferase gene eXpression [CALUX]) were performed on
Table 1 – Year banned and ADI or TDI or PTDI of
those samples. Ten locations presenting a special interest
compounds investigated in this study.
were selected for further analysis of dioxins and dioxin-like
Compounds Year of ban ADI/TDI/PTDI
PCBs by HRGC-HRMS, polybrominated dioxins, polybromi-
(Law 25 Mai 2005;
nated biphenyls and PCB metabolites in eggs, soil, excreta and
VITO, 2007)
feed. A questionnaire was filled out with the help of the hen
PCB (markers) 1986 – owners in order to get information on the hens, the egg
HCH Still used for veterinary ADI: 5 µg/kg bw
consumption and the living environment (possible contam-
purposes (JMPR, 2002)
ination sources, state of the hen house, percentage of soil
HCB 1974 TDI: 0.17 µg/kg bw
(ATSDR, 2002) covered with grass, etc…).
Heptachlor 1976 PTDI: 0.1 µg/kg bw
(heptachlor+ 2.2. Analysis
heptachlorepoxide)
(JMPR, 1994) Details of the analysis are given elsewhere (Van Overmeire
Aldrin/dieldrin 1974 for agricultural use PTDI: 0.1 µg/kg bw
et al., 2006), and the methods are only briefly described in this
1976 for all applications (JMPR, 1994)
paper. All analyses were performed under accreditation,
Chlordane 1981 for agricultural use PTDI: 0.5 µg/kg bw
1998 for all applications (JMPR, 1994) following the 17025 ISO norm.
Endrin Never authorized in PTDI: 0.1 µg/kg bw
Belgium (JMPR, 1994) 2.3. Extraction
Methoxychlor 2003
Nitrofen 1979 in Europe The extraction conditions are described in detail in the paper
(79/117/EEC)
of Van Overmeire et al. (2009). The extraction conditions are
DDT 1974 for agricultural use PTDI: 10 µg/kg bw
1976 for all applications (sum DDT, DDE, DDD)
optimized for the each matrix, as developed during validation
(JMPR, 2000) of the analytical methods. For the eggs, the fat was extracted
with hexane and acetone, the extract was filtrated and dried
ADI: Acceptable Daily Intake; TDI: Tolerable Daily Intake; PTDI:
on a column filled with celite and Na2SO4. Kitchen waste was
Provisional Tolerable Daily Intake.
mixed with 20 mL toluene and 4.5 mL MeOH and shaken for
4432 S CI EN CE OF T H E T OTAL EN V I RO N M EN T 4 0 7 ( 2 0 09 ) 44 3 0–4 43 7

2 h. Soils and excreta were extracted by ASE with toluene


(150 °C, 2000 PSI, 2 cycles of 5 min). 3. Results

2.4. Purification and detection The concentrations of the following compounds have been
determined in 40 egg samples collected in the autumn and in 59
For PCBs, marker PCBs (PCB 28, 52, 101, 118, 153, 138, 180) were eggs samples collected in the spring: hexachlorohexane (α-HCH,
determined by GC-ECD and GC-MS/MS (for confirmation). A β-HCH, γ-HCH), hexachlorobenzene (HCB), heptachlor, hepta-
total of 0.4 g fat was dissolved in hexane, and PCB 143 was chlorepoxide, aldrin, dieldrin, endosulfan, α-chlordane, γ-chlor-
added to control the purification step. The extract was purified dane, oxychlordane, transnanochlor, endrin, methoxychlor,
on a column comprising 6 g acidic silica 40% w/w, 1 g alumina nitrofen, DDT (o,p′-DDT, p,p′-DDT, o,p′-DDE, p,p′DDE, o,p′-DDD,
deactivated with 8% water and 0.5 g sodium sulfate anhydrous. p,p′-DDD), PCB 28, 52, 101, 118, 153, 138, 180.
PCBs were eluted with 20 mL hexane. The extract was spiked Among these samples, the ten most relevant locations
with mirex as an internal standard, concentrated to 1 mL and were chosen for further analysis of the same contaminants in
analyzed by GC-ECD equipped with HT-8 GC column (25 m, soils, feed and excreta (see Van Overmeire et al., 2009 for
0.22 mm × 0.25 µm). PCB results above the maximum residue details of sampling strategy).
level (Royal order, 2000a) were confirmed by GC-MS/MS, an ion-
trap Polaris-Q from Thermo-Finnigan equipped with the same 3.1. Chlorinated pesticides and PCBs in eggs
GC column. For PCBs not detected, a concentration of 0 ng/g fat
was used for the calculation of the sum PCBs, for isomers For a simpler interpretation, only the data obtained for spring
detected but under the limit of quantification (LOQ), a are discussed in this section since eggs were collected at the
concentration of LOQ/2 is used for the calculation of the sum same locations in spring and autumn. Details of the results for
PCBs (LOQ for eggs: 10 ng/g fat; LOQ for soil, excreta and kitchen spring and autumn can be found in the Supplementary data
waste: 2 ng/g). and the comparison between spring and autumn's results can
For pesticides, the following organochlorinated pesticides (OC) be found in the Discussion section.
were analyzed: hexachlorohexane (α-HCH, β-HCH, γ-HCH), hexa- Levels of chlorinated pesticides and PCBs in eggs are
chlorobenzene (HCB), heptachlor, heptachlorepoxide, aldrin, diel- presented and compared to the Belgian norms (Royal order,
drin, endosulfan, α-chlordane, γ-chlordane, oxychlordane, 2000a,b) in Figs. 1 and 2. The norms are expressed in ng/g fat
transnanochlor, endrin, methoxychlor, nitrofen, DDT (o,p′-DDT, for eggs when the percentage of fat is above 10%, as is the case
p,p′-DDT, o,p′-DDE (dichlorodiphenyldichloroethylene), p,p′DDE, for the eggs in this study.
o,p′-DDD (dichlorodiphenyldichloroethane), p,p′-DDD). A total of Until now, there is no European norm for PCBs in eggs;
0.2 g fat was dissolved in hexane, and dibromoctafluorobi- however, a Belgian norm of 200 ng/g fat was set during the
phenyl was added to control the purification step. The extract PCB/dioxin crisis in 1999 for the sum of PCB 28, 52, 101, 118,
was purified on a column comprising 10 g alumina deacti- 153, 138, 180. Two samples are a little bit above this norm, the
vated with 8% water and 0.5 g sodium sulfate anhydrous. OC other samples being usually less than 100 ng/g fat.
are eluted with 80 mL hexane. The extract is spiked with DDT or its metabolites are detected in 95% of the eggs
mirex as an internal standard, concentrated to 1 mL and collected in the spring, and 17% of the samples are above the
analyzed by GC-ECD equipped with two GC columns: an HT-8 norm of 500 ng/g fat. The level found in one sample is
GC column (25 m, 0.22 mm × 0.25 µm) and a DB1701 extremely high, with a concentration of 12,170 ng/g fat.
(60 m × 0.32 mm × 0.25 µm) and two ECD detectors. The For the sum of chlordane (α-chlordane, γ-chlordane,
identity of all OC detected is confirmed by the retention oxychlordane, transnanochlor), two samples are above the
time on the 2 columns. For isomers not detected, a Belgian norm of 50 ng/g fat, but these compounds are not
concentration of 0 ng/g fat was used for the calculation of detected in 64% of the samples. α- and γ-chlordane were
the sum DDT; for isomers detected but under the LOQ, a detected in only one sample of 59, oxychlordane and
concentration of LOQ/2 is used for the calculation of the sum transnanochlor being responsible for the more elevated values
DDT (LOQ for eggs: 10 ng/g fat; LOQ for soil, excreta and measured. The same kind of observation can be made for the
kitchen waste: 2 ng/g). sum of aldrin and dieldrin: three samples above the norm of
200 ng/g fat, but no detection in 49% of the samples. The
2.5. Quality control concentration of aldrin was always under the limit of
quantification.
All analytical methods are under accreditation and strict The other pesticides hexachlorohexane, endosulfan, end-
quality control criteria are applied. A blank sample spiked with rin, methoxychlor and nitrofen were not detected in any
the compounds of interest is analyzed within each series of sample.
samples. Results are plotted on a control chart for which
classical criteria are applied. A procedural blank is analyzed 3.2. Chlorinated pesticides and PCBs in soil, feed and
within each series of samples. None of the compounds excreta
analyzed can be detected in the procedural blank. For PCB
analysis, the percentage recovery of the 13C labeled PCBs must Concentrations measured in eggs, soil, feed and excreta for the
be N50%. For OC analysis, the percentage recovery of the ten selected locations are presented in Table 2 for PCBs and in
surrogate must be in the range 60–120% for fat and in the range Table 3 for DDT. Details of the congener concentrations can be
50–110% for matrix which needs an extraction step. found in the Supplementary data.
S CI EN C E OF TH E T OTAL EN V I RO N M EN T 4 0 7 ( 2 0 09 ) 44 3 0–4 43 7 4433

Fig. 1 – Concentrations of the sum PCB and the sum chlordanes in Flanders and Wallonia.

The pesticides hexachlorohexane, endosulfan, endrin, egg samples from private owners obtained in the previous study
methoxychlor, nitrofen and chlordane have not been detected (Van Overmeire et al., 2006). This level is clearly higher than in
in any sample. Aldrin and dieldrin are detected in sample VB4 eggs from a commercial farm for which the median level
at quite high level (253 ng/g for soil and 42 ng/g for excreta), measured in Belgium was zero (max 63.2 ng/g fat) (Van
and at trace level in a few samples. Traces of HCB are found in Overmeire et al., 2006). This observation is in agreement with
soils collected in spring. other publications (Tlustos et al., 2004; Voorspoels et al., 2008).
Most of the PCBs present in feed is absorbed (~90%) through
the hen's gut. Foraging hens ingest soil particles, and soil can
4. Discussion be a nonnegligible source of contaminants. However, a smaller
percentage of PCBs is actually absorbed from soil than feed
4.1. PCBs because of the stronger adsorption of PCBs on soil particles
(Van Eijkeren et al., 2006).
The median of PCB concentrations in eggs for the whole set of PCB 153 and/or 138 and/or 180 are detected in almost all egg
data is 15.0 ng/g fat for eggs collected in the spring and 32.6 ng/g samples (92%) while PCB 28 is never detected, and PCB 52 and
fat for eggs collected in the autumn. These concentrations agree 101 which are rapidly metabolized (De Vos et al., 2005) are
well with the median of 32.3 ng/g fat found for the analysis of 22 detected in only one sample out of 59.

Fig. 2 – Concentrations of the sum aldrin/dieldrin and the sum DDT in Flanders and Wallonia.
4434 S CI EN CE OF T H E T OTAL EN V I RO N M EN T 4 0 7 ( 2 0 09 ) 44 3 0–4 43 7

Table 2 – Results for the 10 selected locations for the sum of PCBs 28, 52, 101, 118, 153, 138, and 180.
Sum marker PCBs

Sample Eggs ng/g fat Soil ng/g Excreta ng/g Kitchen waste ng/g

Autumn Spring Autumn Spring Autumn Spring Autumn Spring

VB4 345.6 235.5 7.5 5.2 5.9 4.0 5.7 NA


OV3 10.0 0.0 2.6 5.0 4.7 1.0 NA NA
WV1 109.7 66.4 3.7 1.0 5.9 2.0 NA 3.0
LB1 10.0 10.0 3.5 1.0 9.9 1. NA 1.0
A2 41.5 102.5 6.4 2.0 4.9 2.0 11.4 1.0
WB1 10.0 10.0 3.3 0.00 4.3 2.0 NA 2.0
H1 21.4 59.7 7.0 4.0 56.3 4.0 NA NA
H5 39.2 27.0 3.2 0.0 4.9 1.0 2.9 & 4.2 0.0
N2 52.3 5.0 4.9 2.0 NA NA NA NA
L3 26.8 0.0 NA 0.00 3.7 2.0 4.8 NA

NA: Not analyzed; for not detected PCB congeners, a concentration of 0 ng/g fat was used for the calculation of the PCB sum; for isomers detected
but under the LOQ, a concentration of LOQ/2 was used for the calculation of the PCB sum (LOQ for eggs: 10 ng/g fat; LOQ for soil, excreta and
kitchen waste: 2 ng/g).

In order to identify the origin of contamination, soils and to a low PCB contamination of home-produced eggs. Lower
feed were analyzed at ten selected locations. PCBs were concentrations are found in the eggs produced in battery in
detected at low levels in all soil samples, but no clear commercial farm because of the strict control of the feed and
correlation between the soil and egg levels could be estab- to the fact that there is no contact between the environment
lished. For example, the levels in soil for VB4 and OV3 are very (especially the soil) and the hens. The same observation has
close (5.2 and 5.0 ng/g), but the levels in eggs are, respectively, been made several times for dioxins and dioxin-like PCBs
235.5 and 0 ng/g fat. This may be related to differences in (Stephens et al., 1995; Schuler et al., 1997; Harnly et al., 2000;
origin of the contamination, the presence of very local hot Pless-Mulloli et al., 2001; Van Overmeire et al., 2006; Diletti
spots, the bioavailability of PCB which is different from one et al., 2005).
soil to the other (Hawthorne and Grabanski, 2000; Hawthorne The PCB level in Flanders is clearly higher than in Wallonia
and Miller, 2003) and to the amount of soil ingested by the (Fig. 1). These results are in contrast with a study on human
hens which is strongly dependent on the grass coverage of the milk contamination in Belgium, where slightly higher levels in
garden. human milk were found in Wallonia compared to Flanders
Traces of PCBs were found in two kitchen waste samples. (VITO, 2007).
However, the kitchen wastes are different from one owner to
another and vary with time for the same owner. It is then 4.2. DDT
difficult to evaluate the true income of PCBs via the feed from
the data obtained. The median concentration of DDT in eggs is 63.4 ng/g fat, and
There is a general low background of PCBs in soil and, the mean is 457.2 ng/g fat, close to the norm of 500 ng/g fat
probably, in feed. As a consequence, low levels of PCBs are (17% of the samples are above the norm).
ingested by foraging hens. About one third of the PCBs According to Furusawa (2002), DDT is rapidly metabolized
ingested arrived in the egg yolk (De Vos et al., 2005), leading to DDE and DDD in a chicken's body. DDD is found only in the

Table 3 – Results for the 10 selected locations for the sum of DDT/DDD/DDE.
Sum DDT/DDD/DDE

Sample Eggs ng/g fat Soil ng/g Excreta ng/g Kitchen waste ng/g

Autumn Spring Autumn Spring Autumn Spring Autumn Spring

VB4 258.5 91.1 18.0 19.3 3.4 0.0 0.0 NA


OV3 21,390.4 12,170.5 66.7 312.8 512.8 550.3 NA NA
WV1 128.7 139.9 45.0 39.9 8.4 14.4 NA 0.0
LB1 112.4 102.4 15.2 26.4 3.5 5.1 0.0 1.0
A2 3117.7 2245.8 471.5 151.7 68.5 85.5 0.0 0.0
WB1 114.4 118.9 13.4 40.6 2.9 1.0 NA 4.9
H1 471.4 317.4 55.0 10.8 23.0 19.5 NA NA
H5 1848.5 596.1 0.0 2.0 0.0 12.3 0.0 0.0
N2 45.5 5.0 3.0 5.7 2.7 3.5 NA NA
L3 17.1 15.5 0.0 0.0 0.0 0.0 0.0 NA

For isomers not detected, a concentration of 0 ng/g fat was used for the calculation of the DDT sum, for isomers detected but under the LOQ, a
concentration of LOQ/2 is used for the calculation of the DDT sum (LOQ for eggs: 10 ng/g fat; LOQ for soil, excreta and kitchen waste: 2 ng/g).
S CI EN C E OF TH E T OTAL EN V I RO N M EN T 4 0 7 ( 2 0 09 ) 44 3 0–4 43 7 4435

liver, and DDE is excreted via the egg. In agreement with this the henhouse compared to the soil and higher proportion of
observation, 60–100% of the total DDT in an egg is due to the p, DDT isomers inside the henhouse (85%) compared to the soil
p′-DDE isomer, and the rest is due to the p,p′-DDT isomer. sample (40%) (see Van Overmeire et al., 2006 for details).
As for PCBs, the source of contamination was investigated In some cases, the historical use of DDT for hens' house
by the analysis of soils and feed at ten selected locations, with treatment against ectoparasites (protection against hen's flea)
the same limitation (efficiency of the kitchen waste sampling, can explain, at least in part, the high levels found in eggs. In
difference in bioavailability, difference in soil ingestion linked this hypothesis, the henhouse can be considered as the main
to grass coverage). No DDT was found in the kitchen waste, source of contamination. This would explain the high
except a trace in one sample. Concentrations in the soils percentage of p,p′-DDT in soil samples and the absence of
varied between 0 and 471 ng/g (there is no norm for DDT level any correlation between soil and egg levels.
in soils). Again, no direct correlation can be made between egg Nevertheless, a high level of DDT was already measured in
and soil levels. For soil samples, the ratio between p,p′-DDT great tit (residential songbird) eggs in Flanders, in the same
and total DDT is 0.6–0.76. range as that of our samples: 500–2500 ng/g fat (Van den Steen
The decrease of DDT concentration in the environment and et al., 2008). High levels in predatory birds in Belgium were also
human milk marks a general trend since the ban of this reported by Jaspers et al. (2006). As already observed in a study
product years ago (Smith, 1999; VITO, 2007). And, indeed, DDT on human milk contamination in Belgium (VITO, 2007), higher
is usually not detected anymore or only at trace level in DDT levels are found in Flanders compared to Wallonia (Fig. 2).
commercial eggs, as observed in Spain (Fontcuberta et al.,
2008), in Belgium (17.30 ng/g fat) (Van Overmeire et al., 2006) or 4.3. Other chlorinated pesticides
in Sweden (6.6 ng/g fat) (Darnerud et al., 2006). The high levels
measured in this study are surprising and raise questions Results for the other chlorinated pesticides are more in
about this pesticide banned for more than 30 years in Belgium. agreement with expected levels for banned compounds: no
As for PCBs, a higher concentration in home-produced eggs traces can be detected in most of the samples, except for a few
is expected, but the levels measured are on the order of one exceptions for aldrin/dieldrin and chlordane.
reported in a region where DDT had been sprayed 9 years
before (Vieira et al., 2001). In this case study, a house was 4.4. Comparison autumn and spring
sprayed with DDT inside and outside the house walls in 1990.
Nine years later, the concentration of DDT in soils close to the Quite good correlation is observed between the DDT concen-
house was 113 ng/g, and the p,p′-DDT isomers represented trations in eggs in autumn and in spring (Fig. 3). The results for
about 35% of the total. The half-life of DDT in soil of temperate OV3 sample is one order of magnitude higher than the other
regions is about 7 years. DDT may be degraded by UV radiation results and was not included in the calculations or in the
and by microorganisms to DDE and DDD. The concentration of graph. Including this result in calculation would raise the
the outside and inside house walls showed much higher correlation coefficient from 0.78 to 0.98 which would not be
concentrations than soil: 1062 and 449 ng/g for the total DDT representative of the data set. Concentrations in autumn are
respectively. The p,p′-DDT represent 50% of the total for the usually higher (y = 1.1918x + 14.8), but not systematically.
outer wall and 84% for the inner wall. These results illustrate A correlation between PCB concentrations in eggs in
the lower degradation rate in walls compared to soil (no autumn and spring is less obvious (y = 0.6576x + 16.682,
microorganisms) and the lower degradation rate inside R2 = 0.43). This is probably related to the low concentrations
compared to outside (no UV). Remarkably, the same observa- measured. The analytical method was developed to determine
tions were made for sample OV3, for which more investiga- samples above the norm of 200 ng/g fat and has LOQ of 10 ng/g
tions were performed because of the extremely high levels in fat for each of the congeners. Since concentrations measured
this sample: higher concentration in the dust collected inside in this study are often close to or below the LOQ (LOQ/2 is used

Fig. 3 – Comparison of DDT concentration in eggs from autumn and spring.


4436 S CI EN CE OF T H E T OTAL EN V I RO N M EN T 4 0 7 ( 2 0 09 ) 44 3 0–4 43 7

Table 4 – Percentage of the Provisional Tolerable Daily egg consumption represents less than 1% of the PTDI for all
Intake (PTDI) due to home-produced egg consumption for samples, except one sample which represents 4%.
the different families. No direct correlation can be established between soil and
Sample DDTs (% PTDI) egg concentrations for PCB and DDT. However, the contact
with soil and the environment is probably responsible for the
VB4 0.03
OV3 3.52 higher concentrations found in home-produced eggs com-
WV1 0.03 pared to commercial production of eggs for which usually no
LB1 0.03 OC or PCB can be detected. In some cases, the historical uses of
A2 0.51 DDT for henhouse treatment against ectoparasites (protection
WB1 0.03 against hen's flea) can explain, at least in part, the high levels
H1 0.13
found in eggs. In this hypothesis, the henhouse can be
H5 0.62
N2 0.02
considered as the main source of contamination.
L3 0.01 The concentrations in Flanders are usually higher than in
Wallonia.

as concentration for congeners detected but under the LOQ),


the concentrations measured are not precise enough to draw Acknowledgement
any conclusions.
This study was funded by the Belgian Federal Public Service of
4.5. Comparison of DDT intake via egg consumption Health, Food Chain Safety and Environment (Project RT-06/9
with PTDI CONTEGG).

Individual egg consumption data at the ten selected locations


were gathered by a questionnaire (number of eggs consumed
Appendix A. Supplementary data
per week and per member of the family). The number of eggs
per week was then multiplied by the mean weight of the eggs
Supplementary data associated with this article can be found,
sampled in the family (different for each family), the
in the online version, at doi:10.1016/j.scitotenv.2008.11.063.
concentration of DDT compounds measured in the eggs and
a mean fat percentage per season (measured in the CONTEGG
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